超重力强化O_(3)/Fe(Ⅱ)氧化降解DNT实际废水  

Degradation of Actual Wastewater Containing Dinitrtoluene with O3/Fe(Ⅱ)Oxidation Process Enhanced by High Gravity Technology

作　　者：苗富铭 任高妙 武文莉 尚芮泽 景佳鑫 刘有智[1] 焦纬洲[1] MIAO Fu-ming;REN Gao-miao;WU Wen-li;SHANG Rui-ze;JING Jia-xin;LIU You-zhi;JIAO Wei-zhou(Shanxi Province Key Laboratory of Higee‑Oriented Chemical Engineering and School of Chemical Engineering and TechnologyNorth University of China,Taiyuan 030051,China)

机构地区：[1]中北大学超重力化工过程山西省重点实验室,化学工程与技术学院,山西太原030051

出　　处：《含能材料》2022年第10期995-1003,共9页Chinese Journal of Energetic Materials

基　　金：山西省高等学校科技成果转化培育项目(2020CG040);山西省“1331工程”提质增效建设计划(nuc2021‑006)。

摘　　要：二硝基甲苯(DNT)生产工艺中产生的废水具有成分复杂、难生物降解等特点,为此本研究提出采用超重力强化O_(3)/Fe(Ⅱ)氧化降解DNT实际废水的思路,研究了操作参数对DNT废水去除效果的影响规律,揭示了超重力强化O_(3)/Fe(Ⅱ)氧化降解DNT的催化机理,分析了DNT降解过程中间产物,推测了其降解途径。结果表明:超重力因子的提高有利于硝基化合物的深度降解,体系pH值会影响臭氧的直接氧化和间接氧化反应以及催化剂Fe(Ⅱ)的浓度,在超重力因子β为40,Fe(Ⅱ)浓度为0.8 mmol·L^(-1),O_(3)浓度为60 mg·L^(-1),液体流量QL为80 L·h^(-1),pH值为1.1的条件下,反应60 min硝基化合物的去除率达60%,相近操作条件下,硝基化合物去除率比鼓泡反应器(BR)O_(3)/Fe(Ⅱ)体系提高18.30%;电子顺磁共振图谱显示出1∶2∶2∶1的相对峰强度,表明了羟基自由基(·OH)的存在,证实该降解过程遵循·OH的催化机理;旋转填料床(RPB)O_(3)/Fe(Ⅱ)体系中降解DNT过程的中间产物主要有二硝基苯甲醛、二硝基苯甲酸、二硝基苯、间苯二酚和丙二酸,并推测了Fe(Ⅱ)催化臭氧氧化二硝基甲苯的降解途径。The wastewater generated in the production process of dinitrotoluene(DNT)is characterized by complex composition and difficult biodegradation.In this study,the idea of O_(3)/Fe(Ⅱ)oxidation enhanced by high gravity to degrade actual DNT wastewater was proposed.The effect of operating parameters on DNT wastewater removal was studied,and the catalytic mechanism of O_(3)/Fe(Ⅱ)oxidation degradation of DNT enhanced by high gravity was revealed.The intermediate products in DNT degradation process were analyzed,and the degradation pathway was speculated.The results showed that the increase of the high gravity factor facilitated the deep degradation of nitro compounds,and the pH of the system affected the direct and indirect oxidation reactions of ozone and the concentration of catalyst Fe(Ⅱ).Under the conditions of high gravity factor(β)of 40,the Fe(Ⅱ)concentration of 0.8 mmol·L^(-1),the O_(3)concentration of 60 mg·L^(-1),liquid flow(QL)of 80 L·h^(-1)and pH of 1.1,60%of nitro com‑pounds were removed after the reaction for 60 min.Under similar operating conditions,the removal rate of nitro compounds was 18.30%higher than that of the bubbled reactor(BR)O_(3)/Fe(Ⅱ)system.The electron paramagnetic resonance spectrum showed the relative peak intensity of 1∶2∶2∶1,indicating the existence of hydroxyl radical(·OH),confirming that the degradation process followed the catalytic mechanism of·OH.The intermediates of DNT degradation in rotating packed bed(RPB)O_(3)/Fe(Ⅱ)system mainly include dinitrobenzaldehyde,dinitrobenzoic acid,dinitrobenzene,resorcinol,malonic acid.The degradation pathway of Fe(Ⅱ)‑catalyzed ozonation of dinitrotoluene was speculated.

关 键 词：超重力技术 臭氧 高级氧化法 DNT废水 降解途径 

分 类 号：TJ55[兵器科学与技术—军事化学与烟火技术]